Supported Gold Nanoparticles as Efficient Catalysts in the Solventless Plasmon Mediated Oxidation of sec-Phenethyl and Benzyl Alcohol

• Published in: Journal of physical chemistry. C 2013-06, Vol.117 (23), p.12279-12288
• Main Authors: Hallett-Tapley, Geniece L, Silvero, M. Jazmín, Bueno-Alejo, Carlos J, González-Béjar, María, McTiernan, Christopher D, Grenier, Michel, Netto-Ferreira, José Carlos, Scaiano, Juan C
• Format: Article
• Language: English
• Subjects: Applied sciences; Catalytic methods; Collective excitations (including excitons, polarons, plasmons and other charge-density excitations); Condensed matter: electronic structure, electrical, magnetic, and optical properties; Cross-disciplinary physics: materials science; rheology; Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures; Electronics; Exact sciences and technology; Materials science; Methods of nanofabrication; Nanocrystalline materials; Nanoscale materials and structures: fabrication and characterization; Optoelectronic devices; Physics; Semiconductor electronics. Microelectronics. Optoelectronics. Solid state devices; Surface and interface electron states
• ISSN: 1932-7447; 1932-7455
• DOI: 10.1021/jp311069v

Surface plasmon excitation of supported gold nanoparticles in the presence of H2O2 leads to selective oxidation of sec-phenethyl and benzyl alcohols to the carbonyl products acetophenone and benzaldehyde, respectively, in the absence of additional solvents. Light-emitting diodes are compared with microwave irradiation as excitation sources. Hydrotalcite, ZnO, and Al2O3 have been chosen as the solid supports. The overall efficiency of the alcohol oxidation was found to be largely dependent on the nature of the support, with hydrotalcite-derived nanocomposites giving the highest conversions to product, yielding 90% acetophenone after 40 min of LED irradiation. The mechanism for plasmon-mediated alcohol oxidation is believed to involve a significant contribution from the support itself, with adsorption of the alcohol substrate and progression of the oxidation reaction being largely facilitated by the basicity of the support used.